*4.2. Preparation of TO@HNT Hybrid Nanostructure*

The modification of the HNT nanoclay with TO EO was based on a modified evaporation/adsorption process [36]. Firstly, 20 mL of TO was placed in a glass distiller flask and heated at 200 ◦C to remove the D-limonene and L-cymene (see part (1) in Figure 12). The remaining rich in thymol TO was placed in a round bottom glass flask. Above the flask, 2 g of HNT bed was adapted and above the HNT bed, a reflux condenser was placed. With this modified reflux condenser, the remaining rich in thymol TO was heated at 300 ◦C and the evaporated thymol molecules adsorbed on HNT (see part (2) in Figure 12).

When the HNT bed color turned from white to brown the process stopped and the modified HNT was removed and weighted. The wt.%. TO loading to HNT was calculated at approx. 30%. The as-prepared rich in thymol-modified HNT was labeled as TO@HNT and used as active nano-reinforcement in the development of CS/PVOH/TO@HNT active films/coatings.
